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Date

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Thesis Discipline

Chemistry

Degree Grantor

University of Canterbury

Degree Level

Masters

Degree Name

Master of Science

Pollution created by textile dyeing operations attracts significant attention because an effluent containing a complex mixture of coloured and potentially toxic compounds can be released with the discharged water. Developing dyes and dyeing conditions to reduce the amount of residual dye contained in any effluent has been one of many approaches to minimise this environmental impact. However, the presence of coloured discharge cannot be totally eliminated using only this strategy. Thus, development of efficient post-dyeing wastewater treatment methods capable of removing coloured products from the water is of paramount importance.
TiO2-mediated photocatalytic degradation of organic dye molecules via oxidation is the focus of the study reported in this thesis. TiO₂ significantly increases the rate of photodegradation of a wide range of organic dyes under mild operating conditions, and is able to mineralise a wide spectrum of organic contaminants. TiO₂ is also one of the very few substances appropriate for the industrial applications.
One of primary aims of this thesis is to test the hypothesis that augmenting standard TiO₂ photocatalysts with Au nanoparticles could increase performance of a catalyst, while immobilizing TiO₂ on SiO₂ support may improve the cost of the process efficiency, i.e. more photocatalytic degradation per particle of TiO₂. Combining TiO₂ doped with gold nanoparticles on SiO₂ support has the potential to provide the highest photocatalytic ability at the lowest cost.
The first half of the thesis is concerned with establishing and optimizing experimental conditions for monitoring photodegradation via UV-Visible spectroscopy. Effects of various conditions such as temperature, sequence of addition of reagents, exposure to light vs. experiments in dark, sampling methods, and the use of quenching agent were examined.
The main conclusions from this study are that light-induced photodegradation using titanium dioxide nanoparticles catalysts is comparatively more efficient than purely chemical catalytic (e.g. non-light mediated) degradation, even if the latter is performed at elevated temperature. Further, the rate of dye degradation is affected considerably by the parameters of the system.
The degradation rate depends strongly on the pH of the solution, due to charges on both the catalyst surface and in the dye. In general, at pH ≤ 6.8, which is the zero charge point for TiO₂, reactions proceeded faster than those at higher pH. Six dyes from four different classes of dyes used in industry were used in this study, and all showed different photodegradation behaviour.
The second half of thesis tests the photocatalytic abilities of various TiO₂-based catalysts: pure TiO₂ (commercial and custom-made in our laboratory), TiO₂-supported gold nanoparticles (Au/TiO₂), SiO₂-supported TiO₂ (TiO₂/SiO₂), and SiO₂-supported Au/TiO₂. The best photocatalytic performance was observed for the custom-made TiO₂ code-named as e-TiO₂, which was synthesized using the sol-gel method in dry ethanol. TiO₂-supported Au55 nanoparticles showed a similar level of catalytic ability but are significantly more expensive. It was observed that dye adsorption played a significant role in the case of SiO₂-immobilized photocatalysts.